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- ItemProbing multiphoton light-induced molecular potentials([London] : Nature Publishing Group UK, 2020) Kübel, M.; Spanner, M.; Dube, Z.; Naumov, A.Yu.; Chelkowski, S.; Bandrauk, A.D.; Vrakking, M.J.J.; Corkum, P.B.; Villeneuve, D.M.; Staudte, A.The strong coupling between intense laser fields and valence electrons in molecules causes distortions of the potential energy hypersurfaces which determine the motion of the nuclei and influence possible reaction pathways. The coupling strength varies with the angle between the light electric field and valence orbital, and thereby adds another dimension to the effective molecular potential energy surface, leading to the emergence of light-induced conical intersections. Here, we demonstrate that multiphoton couplings can give rise to complex light-induced potential energy surfaces that govern molecular behavior. In the laser-induced dissociation of H2+, the simplest of molecules, we measure a strongly modulated angular distribution of protons which has escaped prior observation. Using two-color Floquet theory, we show that the modulations result from ultrafast dynamics on light-induced molecular potentials. These potentials are shaped by the amplitude, duration and phase of the dressing fields, allowing for manipulating the dissociation dynamics of small molecules.
- ItemXUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment([London] : Nature Publishing Group UK, 2015) Marciniak, A.; Despré, V.; Barillot, T.; Rouzée, A.; Galbraith, M.C.E.; Klei, J.; Yang, C.-H.; Smeenk, C.T.L.; Loriot, V.; Nagaprasad Reddy, S.; Tielens, A.G.G.M.; Mahapatra, S.; Kuleff, A.I.; Vrakking, M.J.J.; Lépine, F.Highly excited molecular species are at play in the chemistry of interstellar media and are involved in the creation of radiation damage in a biological tissue. Recently developed ultrashort extreme ultraviolet light sources offer the high excitation energies and ultrafast time-resolution required for probing the dynamics of highly excited molecular states on femtosecond (fs) (1 fs=10−15s) and even attosecond (as) (1 as=10−18 s) timescales. Here we show that polycyclic aromatic hydrocarbons (PAHs) undergo ultrafast relaxation on a few tens of femtoseconds timescales, involving an interplay between the electronic and vibrational degrees of freedom. Our work reveals a general property of excited radical PAHs that can help to elucidate the assignment of diffuse interstellar absorption bands in astrochemistry, and provides a benchmark for the manner in which coupled electronic and nuclear dynamics determines reaction pathways in large molecules following extreme ultraviolet excitation.
- ItemAttosecond time-resolved photoelectron holography([London] : Nature Publishing Group UK, 2018) Porat, G.; Alon, G.; Rozen, S.; Pedatzur, O.; Krüger, M.; Azoury, D.; Natan, A.; Orenstein, G.; Bruner, B.D.; Vrakking, M. J.J.; Dudovich, N.Ultrafast strong-field physics provides insight into quantum phenomena that evolve on an attosecond time scale, the most fundamental of which is quantum tunneling. The tunneling process initiates a range of strong field phenomena such as high harmonic generation (HHG), laser-induced electron diffraction, double ionization and photoelectron holography - all evolving during a fraction of the optical cycle. Here we apply attosecond photoelectron holography as a method to resolve the temporal properties of the tunneling process. Adding a weak second harmonic (SH) field to a strong fundamental laser field enables us to reconstruct the ionization times of photoelectrons that play a role in the formation of a photoelectron hologram with attosecond precision. We decouple the contributions of the two arms of the hologram and resolve the subtle differences in their ionization times, separated by only a few tens of attoseconds.
- ItemOnset of Bloch oscillations in the almost-strong-field regime([London] : Nature Publishing Group UK, 2022-12-13) Reislöhner, Jan; Kim, Doyeong; Babushkin, Ihar; Pfeiffer, Adrian N.In the field of high-order harmonic generation from solids, the electron motion typically exceeds the edge of the first Brillouin zone. In conventional nonlinear optics, on the other hand, the excursion of band electrons is negligible. Here, we investigate the transition from conventional nonlinear optics to the regime where the crystal electrons begin to explore the first Brillouin zone. It is found that the nonlinear optical response changes abruptly already before intraband currents due to ionization become dominant. This is observed by an interference structure in the third-order harmonic generation of few-cycle pulses in a non-collinear geometry. Although approaching Keldysh parameter γ = 1, this is not a strong-field effect in the original sense, because the iterative series still converges and reproduces the interference structure. The change of the nonlinear interband response is attributed to Bloch motion of the reversible (or transient or virtual) population, similar to the Bloch motion of the irreversible (or real) population which affects the intraband currents that have been observed in high-order harmonic generation.
- ItemIn situ single-shot diffractive fluence mapping for X-ray free-electron laser pulses([London] : Nature Publishing Group UK, 2018) Schneider, Michael; Günther, Christian M.; Pfau, Bastian; Capotondi, Flavio; Manfredda, Michele; Zangrando, Marco; Mahne, Nicola; Raimondi, Lorenzo; Pedersoli, Emanuele; Naumenko, Denys; Eisebitt, StefanFree-electron lasers (FELs) in the extreme ultraviolet (XUV) and X-ray regime opened up the possibility for experiments at high power densities, in particular allowing for fluence-dependent absorption and scattering experiments to reveal non-linear light-matter interactions at ever shorter wavelengths. Findings of such non-linear effects are met with tremendous interest, but prove difficult to understand and model due to the inherent shot-to-shot fluctuations in photon intensity and the often structured, non-Gaussian spatial intensity profile of a focused FEL beam. Presently, the focused beam is characterized and optimized separately from the actual experiment. Here, we present the simultaneous measurement of XUV diffraction signals from solid samples in tandem with the corresponding single-shot spatial fluence distribution on the actual sample. Our in situ characterization scheme enables direct monitoring of the sample illumination, providing a basis to optimize and quantitatively understand FEL experiments.
- ItemFew-cycle laser driven reaction nanoscopy on aerosolized silica nanoparticles([London] : Nature Publishing Group UK, 2019) Rupp, Philipp; Burger, Christian; Kling, Nora G; Kübel, Matthias; Mitra, Sambit; Rosenberger, Philipp; Weatherby, Thomas; Saito, Nariyuki; Itatani, Jiro; Alnaser, Ali S.; Raschke, Markus B.; Rühl, Eckart; Schlander, Annika; Gallei, Markus; Seiffert, Lennart; Fennel, Thomas; Bergues, Boris; Kling, Matthias F.Nanoparticles offer unique properties as photocatalysts with large surface areas. Under irradiation with light, the associated near-fields can induce, enhance, and control molecular adsorbate reactions on the nanoscale. So far, however, there is no simple method available to spatially resolve the near-field induced reaction yield on the surface of nanoparticles. Here we close this gap by introducing reaction nanoscopy based on three-dimensional momentum-resolved photoionization. The technique is demonstrated for the spatially selective proton generation in few-cycle laser-induced dissociative ionization of ethanol and water on SiO2 nanoparticles, resolving a pronounced variation across the particle surface. The results are modeled and reproduced qualitatively by electrostatic and quasi-classical mean-field Mie Monte-Carlo (M3C) calculations. Reaction nanoscopy is suited for a wide range of isolated nanosystems and can provide spatially resolved ultrafast reaction dynamics on nanoparticles, clusters, and droplets.
- ItemRaman gas self-organizing into deep nano-trap lattice([London] : Nature Publishing Group UK, 2016) Alharbi, M.; Husakou, A.; Chafer, M.; Debord, B.; Gérôme, F.; Benabid, F.Trapping or cooling molecules has rallied a long-standing effort for its impact in exploring new frontiers in physics and in finding new phase of matter for quantum technologies. Here we demonstrate a system for light-trapping molecules and stimulated Raman scattering based on optically self-nanostructured molecular hydrogen in hollow-core photonic crystal fibre. A lattice is formed by a periodic and ultra-deep potential caused by a spatially modulated Raman saturation, where Raman-active molecules are strongly localized in a one-dimensional array of nanometre-wide sections. Only these trapped molecules participate in stimulated Raman scattering, generating high-power forward and backward Stokes continuous-wave laser radiation in the Lamb-Dicke regime with sub-Doppler emission spectrum. The spectrum exhibits a central line with a sub-recoil linewidth as low as ∼14 kHz, more than five orders of magnitude narrower than conventional-Raman pressure-broadened linewidth, and sidebands comprising Mollow triplet, motional sidebands and four-wave mixing.
- ItemMulti-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation([London] : Nature Publishing Group UK, 2015) Ferré, A.; Boguslavskiy, A.E.; Dagan, M.; Blanchet, V.; Bruner, B.D.; Burgy, F.; Camper, A.; Descamps, D.; Fabre, B.; Fedorov, N.; Gaudin, J.; Geoffroy, G.; Mikosch, J.; Patchkovskii, S.; Petit, S.; Ruchon, T.; Soifer, H.; Staedter, D.; Wilkinson, I.; Stolow, A.; Dudovich, N.; Mairesse, Y.High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach for the investigation of unaligned polyatomic molecules, using SF6 as an example. We combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Fragment-resolved above-threshold ionization measurements reveal that strong-field ionization opens at least three channels. A shape resonance in one of them is found to dominate the signal in the 20-26 eV range. This resonance induces a phase jump in the harmonic emission, a switch in the polarization state and different dynamical responses to molecular vibrations. This study demonstrates a method for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.
- ItemNanoplasmonic electron acceleration by attosecond-controlled forward rescattering in silver clusters([London] : Nature Publishing Group UK, 2017) Passig, Johannes; Zherebtsov, Sergey; Irsig, Robert; Arbeiter, Mathias; Peltz, Christian; Göde, Sebastian; Skruszewicz, Slawomir; Meiwes-Broer, Karl-Heinz; Tiggesbäumker, Josef; Kling, Matthias F.; Fennel, ThomasIn the strong-field photoemission from atoms, molecules, and surfaces, the fastest electrons emerge from tunneling and subsequent field-driven recollision, followed by elastic backscattering. This rescattering picture is central to attosecond science and enables control of the electron's trajectory via the sub-cycle evolution of the laser electric field. Here we reveal a so far unexplored route for waveform-controlled electron acceleration emerging from forward rescattering in resonant plasmonic systems. We studied plasmon-enhanced photoemission from silver clusters and found that the directional acceleration can be controlled up to high kinetic energy with the relative phase of a two-color laser field. Our analysis reveals that the cluster's plasmonic near-field establishes a sub-cycle directional gate that enables the selective acceleration. The identified generic mechanism offers robust attosecond control of the electron acceleration at plasmonic nanostructures, opening perspectives for laser-based sources of attosecond electron pulses.
- ItemAnisotropic photoemission time delays close to a Fano resonance([London] : Nature Publishing Group UK, 2018) Cirelli, Claudio; Marante, Carlos; Heuser, Sebastian; Petersson, C.L.M.; Galán, Álvaro Jiménez; Argenti, Luca; Zhong, Shiyang; Busto, David; Isinger, Marcus; Nandi, Saikat; Maclot, Sylvain; Rading, Linnea; Johnsson, Per; Gisselbrecht, Mathieu; Lucchini, Matteo; Gallmann, Lukas; Dahlström, J. Marcus; Lindroth, Eva; L’Huillier, Anne; Martín, Fernando; Keller, UrsulaElectron correlation and multielectron effects are fundamental interactions that govern many physical and chemical processes in atomic, molecular and solid state systems. The process of autoionization, induced by resonant excitation of electrons into discrete states present in the spectral continuum of atomic and molecular targets, is mediated by electron correlation. Here we investigate the attosecond photoemission dynamics in argon in the 20-40 eV spectral range, in the vicinity of the 3s -1 np autoionizing resonances. We present measurements of the differential photoionization cross section and extract energy and angle-dependent atomic time delays with an attosecond interferometric method. With the support of a theoretical model, we are able to attribute a large part of the measured time delay anisotropy to the presence of autoionizing resonances, which not only distort the phase of the emitted photoelectron wave packet but also introduce an angular dependence.
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